# Fileset

[jz2023_02466aR2_SI_final.docx](https://mdr.nims.go.jp/filesets/2829b338-2b4d-4522-9313-16d0f73795f1/download)

## Creator

[溝口拓](https://orcid.org/0000-0002-0992-7449), 大沢祐太, 笹瀬雅人, [大橋直樹](https://orcid.org/0000-0002-4011-0031), 北野政明, [細野秀雄](https://orcid.org/0000-0001-9260-6728)

## Rights

This document is the Accepted Manuscript version of a Published Work that appeared in final form in Ammonia cracking catalyzed by Ni nanoparticles confined in the framework of CeO2 support, copyright © 2023 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jpclett.3c02446.[In Copyright](http://rightsstatements.org/vocab/InC/1.0/)

## Other metadata

[Ammonia cracking catalyzed by Ni nanoparticles confined in the framework of CeO2 support](https://mdr.nims.go.jp/datasets/0be97332-d0bd-42e4-960d-7b35849290c1)

## Fulltext

Supporting InformationAmmonia Cracking Catalyzed by Ni Nanoparticles Confined in the Framework of CeO2 SupportHiroshi Mizoguchi,1,Ⅱ,* Yuta Osawa,1,Ⅱ Masato Sasase,2 Naoki Ohashi,3 Masaaki Kitano,2 andHideo Hosono1, 2, *1Research Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS)1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan2MDX Research Center for Element Strategy, International Research Frontiers Initiative, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama 226-8503, Japan3Research Center for Electronic and Optical Materials, National Institute for Materials Science (NIMS)1-1 Namiki, Tsukuba, Ibaraki 305-0044, JapanⅡThese authors contributed equally to this work*Corresponding author footnote: MIZOGUCHI.Hiroshi@nims.go.jp, hosono@mces.titech.ac.jpTable S1. Catalytic performance of Ni-based catalysts for NH3 cracking under 1 atm. Ni wt% support promoter WHSV(mL g-1h-1) GHSV(h-1) T (℃) conv (%) ref 63 CeO2  10000  400 22 This work 72 YO1.5  10000  400 26 This work 58 Al2O3  30000  450 15 1 10 Al2O3  240000 80000 500 93 2 10 Al2O3  9000  400 32 3 58 Al2O3 Ce 30000  450 28 1 5 C   13000 400 19 4 10 GNP  15000 12000 375 17 5 58 Al2O3 La 30000  450 26 6 20 MgO La 22000  400 28 7 7 MCM-41  36000  500 58 8 10 CaNH  15000  400 19 9 Fig. S1. (a) Time course of NH3 cracking over RNi5 (R = Ce or Y). (b) WHSV dependance of the conversion in NH3 cracking over CeNi5. As the WHSV increased, the activity decreased because of the shortening of the contact time between the catalyst and the NH3 molecule.Fig. S2. Insertion and deinsertion of oxygen in CeNi5 to enhance IM thermal decomposition at atomic scale.　　　　　　　　　　　　　　　　　　　　　　　　　　　　　　　 Fig. S3. Halder–Wagner plot of Ni phase in CeNi5 catalyst to determine CS. β is spread of integral peak width.Fig. S4. TDS spectra at a specific mass-to-charge (m/z) of 2 (H2), 17 (NH3), or 28 (N2) for RNi5 catalysts after NH3 reaction (R = Ce (a) or Y (b)).Fig. S5. Temperature dependence of the conversion in NH3 cracking over various Ni-based catalysts at a WHSV of 10000 mLNH3 gcat-1 h-1. The effect of BM is shown. REFERENCES1. Zheng, W.;  Zhang, J.;  Ge, Q.;  Xu, H.; Li, W., Effects of CeO2 Addition on Ni/Al2O3 Catalysts for the Reaction of Ammonia Decomposition to Hydrogen. Appl. Catal. B: Environ. 2008, 80 (1-2), 98-105.2. Simonsen, S. B.;  Chakraborty, D.;  Chorkendorff, I.; Dahl, S., Alloyed Ni-Fe Nanoparticles as Catalysts for NH3 Decomposition. Appl. Catal. A: General 2012, 447-448, 22-31.3. Han, X.;  Chu, W.;  Ni, P.;  Luo, S.; Zhang, T., Promoting Effects of Iridium on Nickel Based Catalyst in Ammonia Decomposition. J. Fuel Chem. Tech. 2007, 35, 691-695.4. Bramwell, P. L.;  Lentink, S.;  Ngene, P.; de Jongh, P. E., Effect of Pore Confinement of LiNH2 on Ammonia Decomposition Catalysis and the Storage of Hydrogen and Ammonia. J. Phys. Chem. C 2016, 120 (48), 27212-27220.5. Chang, F.;  Wu, H.;  Pluijm, R. V.;  Guo, J.;  Ngene, P.; de Jongh, P. E., Effect of Pore Confinement of NaNH2 and KNH2 on Hydrogen Generation from Ammonia. J. Phys. Chem. C Nanomater Interfaces 2019, 123 (35), 21487-21496.6. Zhang, J.;  Xu, H.;  Jin, X.;  Ge, Q.; Li, W., Characterizations and Activities of the Nano-sized Ni/Al2O3 and Ni/La–Al2O3 Catalysts for NH3 Decomposition. Appl. Catal. A: General 2005, 290 (1-2), 87-96.7. Hu, X.;  Wang, W.;  Jin, Z.;  Wang, X.;  Si, R.; Jia, C., Transition Metal Nanoparticles Supported La-Promoted MgO as Catalysts for Hydrogen Production via Catalytic Decomposition of Ammonia. J. Energy Chem. 2019, 38, 41-49.8. Duan, X.;  Qian, G.;  Liu, Y.;  Ji, J.;  Zhou, X.;  Chen, D.; Yuan, W., Structure Sensitivity of Ammonia Decomposition over Ni Catalysts: A Computational and Experimental Study. Fuel Process. Tech. 2013, 108, 112-117.9. Ogasawara, K.;  Nakao, T.;  Kishida, K.;  Ye, T.;  Lu, Y.;  Abe, H.;  Niwa, Y.;  Sasase, M.;  Kitano, M.; Hosono, H., Ammonia Decomposition over CaNH-Supported Ni Catalysts via an NH2--Vacancy-Mediated Mars-van Krevelen Mechanism. ACS Catal. 2021, 11, 11005-11015.S4image2.pngimage3.pngimage4.pngimage5.pngimage1.png